TY - JOUR
T1 - Multicomponent density-functional theory for time-dependent systems
AU - Butriy, O.
AU - Ebadi, H.
AU - De Boeij, P. L.
AU - Van Leeuwen, R.
AU - Gross, E. K.U.
PY - 2007/11/29
Y1 - 2007/11/29
N2 - We derive the basic formalism of density functional theory for time-dependent electron-nuclear systems. The basic variables of this theory are the electron density in body-fixed frame coordinates and the diagonal of the nuclear N -body density matrix. The body-fixed frame transformation is carried out in order to achieve an electron density that reflects the internal symmetry of the system. We discuss the implications of this body-fixed frame transformation and establish a Runge-Gross-type theorem and derive Kohn-Sham equations for the electrons and nuclei. We illustrate the formalism by performing calculations on a one-dimensional diatomic molecule for which the many-body Schrödinger equation can be solved numerically. These benchmark results are then compared to the solution of the time-dependent Kohn-Sham equations in the Hartree approximation. Furthermore, we analyze the excitation energies obtained from the linear response formalism in the single pole approximation. We find that there is a clear need for improved functionals that go beyond the simple Hartree approximation.
AB - We derive the basic formalism of density functional theory for time-dependent electron-nuclear systems. The basic variables of this theory are the electron density in body-fixed frame coordinates and the diagonal of the nuclear N -body density matrix. The body-fixed frame transformation is carried out in order to achieve an electron density that reflects the internal symmetry of the system. We discuss the implications of this body-fixed frame transformation and establish a Runge-Gross-type theorem and derive Kohn-Sham equations for the electrons and nuclei. We illustrate the formalism by performing calculations on a one-dimensional diatomic molecule for which the many-body Schrödinger equation can be solved numerically. These benchmark results are then compared to the solution of the time-dependent Kohn-Sham equations in the Hartree approximation. Furthermore, we analyze the excitation energies obtained from the linear response formalism in the single pole approximation. We find that there is a clear need for improved functionals that go beyond the simple Hartree approximation.
UR - http://www.scopus.com/inward/record.url?scp=36649013454&partnerID=8YFLogxK
U2 - 10.1103/PhysRevA.76.052514
DO - 10.1103/PhysRevA.76.052514
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AN - SCOPUS:36649013454
SN - 1050-2947
VL - 76
JO - Physical Review A - Atomic, Molecular, and Optical Physics
JF - Physical Review A - Atomic, Molecular, and Optical Physics
IS - 5
M1 - 052514
ER -